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    Home > SCI. Adv.: Academician Li can's team realizes high selective and stable hydrogenation of CO2 to methanol

    SCI. Adv.: Academician Li can's team realizes high selective and stable hydrogenation of CO2 to methanol

    • Last Update: 2017-10-17
    • Source: Internet
    • Author: User
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    China's 11th five year plan proposes "energy conservation and emission reduction", in which "emission reduction" refers to reducing emissions The emission of carbon dioxide and other greenhouse gases causes global warming, which has been widely concerned by the international community It is a feasible way to reduce CO2 emission by using solar photocatalytic hydrolysis to produce hydrogen to produce clean fuel such as methanol from CO2 hydrogenation Methanol is not only an important chemical raw material, but also a promising clean fuel The hydrogenation of CO2 to methanol is one of the most effective ways to utilize CO2, which is of great significance to solve the problems of environmental protection and energy Although the CO hydrogenation to methanol has been industrialized, the CO 2 hydrogenation to methanol still faces the problems of low selectivity and poor stability, especially for the supported metal catalyst under industrial conditions Recently, Dr Wang Jijie and Academician Li can from the State Key Laboratory of Catalysis (Dalian Institute of Chemical Physics, Chinese Academy of Sciences) reported a bimetallic ZnO ZrO 2 solid solution oxide catalyst, which realized the highly selective and stable hydrogenation of CO 2 to methanol When the conversion of CO2 is over 10%, the selectivity of methanol is up to 86% to 91%, which is the best result in the same research From the perspective of understanding photosynthesis, the hydrogenation process of CO2 to methanol implies the dark reaction effect in photosynthesis, which is an important way of making liquid fuel from solar energy Academician Li can's team attaches great importance to the utilization of renewable energy to realize the transformation and resource utilization of CO2 Methanol fuel can not only replace gasoline and diesel as internal combustion engine fuel, but also as fuel of fuel cell or new C1 chemical raw material Due to the difficulty of CO 2 activation, the research and development of high efficiency catalyst has become one of the important factors for the industrialization of CO 2 hydrogenation to methanol technology Academician Li can's team has long been committed to the research of solar photocatalysis, photocatalysis and hydrogen production by electrolyzing water In the process of carbon dioxide hydrogenation, improving the selectivity of methanol is also a major challenge for CO2 conversion The research shows that the ZnO ZrO2 Solid Solution oxide catalyst developed by Academician Li can team provides double active catalytic sites Zn and Zr for the reaction, in which H 2 and CO 2 are activated at the Zn site and the Zr site adjacent to the atom respectively, and show a synergistic effect, and can generate methyl alcohol with high selectivity The performance of ZnO ZrO 2 catalyst is closely related to the molar ratio of Zn / (Zn + Zr) When the molar percentage of Zn is 13%, the catalytic activity is significantly enhanced and the highest conversion is achieved The performance of zno-zro 2 catalyst is closely related to the Zn / (Zn + Zr) molar ratio (source: Science Advanced) The experimental results show that the reaction temperature has an obvious effect on the reaction When the reaction temperature was increased, the selectivity of methanol decreased, while the conversion of carbon dioxide increased When the conversion reached 10% at 320 ℃, the selectivity of methanol remained at 86% Temperature affects the selectivity of methanol and the conversion of carbon dioxide (source: Science Advanced) In addition, it is worth noting that the selectivity of methanol and the conversion of carbon dioxide remain at a high level when the reaction continues for more than 500 hours, indicating that the catalyst has not been deactivated Surprisingly, the catalyst also showed some sulfur resistance Sulfur molecules are contained in the flue gas from coal combustion or biomass combustion The sulfur resistance of the ZnO ZrO 2 catalyst will greatly reduce the cost of feed gas purification, and it has a good prospect of industrial application After 500 hours of continuous reaction, the catalyst did not lose its activity (source: Science Advanced) XRD results showed that ZrO2 prepared by coprecipitation method was mainly monoclinic phase and mixed some tetragonal phase The monoclinic phase of zirconium can be transformed into tetragonal or cubic phase by adding ZnO (5-33%) into ZrO2 The XRD pattern of ZnO-ZrO2 (source: Science Advanced) was followed by an evaluation of the formate pathway and the carbon monoxide pathway, the two main pathways of carbon dioxide hydrogenation The DFT results show that the hydrogenation of CO2 * to HCOO * is a positive and beneficial process, which is consistent with the results of diffuse reflectance Fourier transform infrared spectroscopy (DRIFTS) H 2CO * + h * → h 3Co * (△ g ≠ = − 2.32 EV), so h 3Co * is the most stable intermediate Finally, H 3Co * is protonated to form methanol Therefore, it is confirmed that the reaction pathway is formate pathway DFT calculation: CO 2 hydrogenation reaction diagram (energy E and Gibbs free energy g at 593k) (source: Science Advanced) This work has opened a new way for CO 2 hydrogenation to methanol The use of bimetallic ZnO ZrO 2 solid solution oxide catalyst realizes the high selective and stable hydrogenation of CO 2 to methanol, which has a good prospect of industrial application At the same time, the research also reflects the positive contribution of Chinese scientists to the control of the continuous increase of greenhouse gases We believe that through the unremitting efforts of scientists and the masses, we will be able to lead a low-carbon life Paper link: http://advances.sciencemag.org/content/3/10/e1701290
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